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By introducing large counter cations as the spacer, two isolated 3, 3-ladder compounds, (Ph 4 P)[Co II (3-Mepy) 2.7 (H 2 O) 0.3 W V (CN) 8 ]·0.6H 2 O ( 1 ) and (Ph 4 As)[Co II (3-Mepy) 3 W V (CN) 8 ] ( 2 , 3-Mepy = 3-methylpyridine), were synthesized and characterized. Static and dynamic magnetic characterizations reveal that compounds  1  and  2  both behave as the single-chain magnets (SCMs) with very high energy barriers: 252(9) K for  1  and 224(7) K for  2 , respectively. These two compounds display the highest relaxation barriers for cyano-bridged SCMs and are preceded only by two cobalt(II)-radical compounds among all SCMs. Meanwhile, a large coercive field of 26.2 kOe ( 1 ) and 22.6 kOe ( 2 ) were observed at 1.8 K.

Single-Chain Magnets Based on Octacyanotungstate with the Highest Energy Barriers for Cyanide Compounds